Influence of Parameters in Vapor Transport Equilibration Treatment on Composition and Homogeneity of LiTaO3 Single Crystals

Minerva Gonzalez, S. Margueron, Tomas Murauskas, Pascal Boulet, Ludovic Gauthier‐Manuel, Bernard Dulmet, A. Bartasyte
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Abstract

The effect of key parameters such as time, temperature, and equilibration powder concentration in vapor transport equilibration (VTE) treatment on the Li2O content of initially congruent X‐, Y‐, and Z‐cut LiTaO3 crystals is experimentally investigated. The Li2O content across the thickness of the crystal is estimated by Raman spectroscopy with accuracy of 0.05–0.15 mol%. The Li2O loss from equilibration powders has been monitored as a function of treatment temperature and duration. The results show that the Li2O content in the crystal nonlinearly depends on the equilibration powder composition and that homogeneous stoichiometric LiTaO3 crystals can be obtained by treatment for at least 36h at 1250°C in Li2O‐rich atmosphere, created by powders containing >54 mol% of Li2O. The anisotropic Li+ diffusion coefficients and its activation energy are also experimentally estimated. Finally, the VTE conditions are defined for the production of different cuts of LiTaO3 crystals with controlled homogeneous Li2O nonstoichiometry in the range from subcongruent to stoichiometric compositions.
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气相传输平衡处理参数对氧化钽锂单晶成分和均匀性的影响
实验研究了气相传输平衡(VTE)处理中的时间、温度和平衡粉浓度等关键参数对初始全等 X、Y 和 Z 切面 LiTaO3 晶体中 Li2O 含量的影响。通过拉曼光谱估算了晶体厚度上的 Li2O 含量,精确度为 0.05-0.15 摩尔%。根据处理温度和持续时间的函数,对平衡粉末中 Li2O 的损失进行了监测。结果表明,晶体中的 Li2O 含量与平衡粉末成分呈非线性关系,在富含 Li2O 的气氛中于 1250°C 下处理至少 36 小时,可获得均一的 LiTaO3 晶体。实验还估算了各向异性的 Li+ 扩散系数及其活化能。最后,定义了生产不同切割的 LiTaO3 晶体的 VTE 条件,这些晶体具有受控的均匀 Li2O 非全度性,其成分范围从亚全度性到全度性。
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